Interfacial active sites on Co‐Co 2 C@carbon heterostructure for enhanced catalytic hydrogen generation

Abstract Designing catalysts with capable dual‐active sites to drive catalytic hydrogen generation is necessary for the future hydrogen economy. Herein, the interfacial active sites consisting of Co and Co‐C on Co‐Co 2 C@carbon heterostructure are designed through annealing and high‐pressure carbonization. The operating temperature during the high‐pressure carbonization under a CO‐reducing environment is responsible for the construction and regulation of Co‐Co 2 C@C heterostructure. The optimal catalyst has a high turnover frequency (TOF) of 33.1 min −1 and low activation energy ( E a ) of 27.3 kJ·mol –1 during the hydrolysis of NH 3 BH 3 . The catalytic stability of Co‐Co 2 C@C has no dramatic deterioration even after 5 cyclic usages. The interfacial active sites and the carbon on the catalyst surface enhance hydrogen generation kinetics and catalytic stability. The construction of interfacial active sites in Co‐Co 2 C@C prompts the dissociation of reactants (NH 3 BH 3 and H 2 O molecules), leading to an enhanced catalytic hydrogen generation from NH 3 BH 3 hydrolysis (Co activates NH 3 BH 3 and Co‐C activates H 2 O). The construction of hetero‐structural catalysts provides theoretical direction for the rational design of advanced transition metal carbide materials in the field of energy catalysis and conversion.